Beyond PXRD Pattern Matching: Toward Rigorous Structure Determination in Covalent Organic Frameworks

Abstract

ABSTRACT Widespread reliance on qualitative powder x‐ray diffraction (PXRD) pattern matching has led to systematic overinterpretation of covalent organic framework (COF) structures. As a result, structure–property relationships are often obscured, mechanistic conclusions can be misleading, and reported performance is not always reproducible. In this Perspective, we take a closer look at common weaknesses in current practice, focusing on mismatches between proposed structural models and the characterization data used to support them. Through representative case studies, we show how these inconsistencies arise and why they matter. We argue that more rigorous, evidence‐based approaches, achieved via complementary characterization techniques, are needed for reliable structure determination. We also emphasize the importance of transparent data reporting and deposition, and introduce a practical checklist to help authors, reviewers, and editors assess the strength of structural claims in COFs.